期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 52, 页码 27126-27134出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202112870
关键词
electrocatalytic water splitting; iridium clusters; lattice oxygen oxidation mechanism; metal borides; oxygen evolution reaction
资金
- National Natural Science Foundation of China [21972015, 22088102, 12074053]
- Young top talents project of Liaoning Province [XLYC1907147, XLYC1907163]
- Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science [2019JH3/30100003]
- Fundamental Research Funds for the Central Universities [DUT20TD06]
- Liaoning Revitalization Talent Program [XLYC2008032]
This study reports an efficient oxygen evolution reaction (OER) catalyst that combines iridium clusters and high-valence cobalt species, achieving non-concerted proton-electron transfer at the atomic scale to trigger OER activity at multiple active sites. Experimental evidence confirms the importance of lattice oxygen oxidation mechanism, while theoretical simulations suggest that the catalyst's OER performance is mainly dominated by the LOM pathway, facilitating reaction kinetics.
Developing robust oxygen evolution reaction (OER) catalysts requires significant advances in material design and in-depth understanding for water electrolysis. Herein, we report iridium clusters stabilized surface reconstructed oxyhydroxides on amorphous metal borides array, achieving an ultralow overpotential of 178 mV at 10 mA cm(-2) for OER in alkaline medium. The coupling of iridium clusters induced the formation of high valence cobalt species and Ir-O-Co bridge between iridium and oxyhydroxides at the atomic scale, engineering lattice oxygen activation and non-concerted proton-electron transfer to trigger multiple active sites for intrinsic pH-dependent OER activity. The lattice oxygen oxidation mechanism (LOM) was confirmed by in situ O-18 isotope labeling mass spectrometry and chemical recognition of negative peroxo-like species. Theoretical simulations reveal that the OER performance on this catalyst is intrinsically dominated by LOM pathway, facilitating the reaction kinetics. This work not only paves an avenue for the rational design of electrocatalysts, but also serves the fundamental insights into the lattice oxygen participation for promising OER application.
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